Resonance ionization spectroscopy and one-atom detection

Abstract

Resonance ionization spectroscopy, RIS, is a multistep photon absorption process in which the final state is the ionization continuum of an atom. The RIS process can be saturated with available pulsed lasers, so that one electron can be removed from each atom of the selected type. This method was first applied to the determination of the absolute number of He($2^{1}S$) excited states produced when pulsed beams of protons interacted with helium gas. Laser schemes for RIS are classified into five basic types; with these, nearly all of the elements can be detected with commercially available lasers. A periodic table is included showing schemes applicable to all of the elements except He, Ne, F, and Ar. A compact theory of the RIS process is presented which delineates the conditions under which rate equations apply. Questions on the effects of collisional line broadening, laser coherence time, and nonresonant multiphoton ionization processes are discussed. The initial demonstration of one-atom detection of Cs is described. By using laser beams to saturate the RIS process and by using proportional counters as single-electron detectors, one-atom detection is made possible. With RIS, one-atom detection is highly selective, has the ultimate in sensitivity, and has excellent space and time resolution. Furthermore, a modification of the technique in which single electrons (or single ions) are detected with a channel electron multiplier permits single-atom detection in a vacuum. Resonance ionization spectroscopy has application to classical phenomena such as the diffusion of free atoms, the chemical reaction of free atoms with a gas, the measurement of concentration fluctuations in a dilute vapor, and a variety of other atomic fluctuation phenomena. The authors describe how RIS can be used for photophysics measurements such as far wing collisional line broadening, measurements of photoionization cross sections for excited states, and collisional redistribution among excited states. Modern applications include the detection of single atoms in individual ionization tracks, such as those created by the binary fission of a parent atom, and the extension of this technique to the detection of stable or unstable daughter atoms in time coincidence with the decay of a parent atom. These methods are beig developed for use in low-level counting to determine, for example, the flux of solar neutrinos on the earth.